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The Hubbard model is believed to capture the essential physics of cuprate superconductors. However, recent theoretical studies suggest that it fails to reproduce a robust and homogeneous superconducting ground state. Here, using resonant inelastic x-ray scattering and density matrix renormalization group calculations, we show that magnetic excitations in the prototypical cuprate ladder Sr$_{14}$Cu$_{24}$O$_{41}$ are inconsistent with those of a simple Hubbard model. The magnetic response of hole carriers, contributing to an emergent branch of spin excitations, is strongly suppressed. This effect is the consequence of d-wave-like pairing, enhanced by nearly an order of magnitude through a large nearest-neighbor attractive interaction. The similarity between cuprate ladders and the two-dimensional compounds suggests that such an enhanced hole pairing may be a universal feature of superconducting cuprates., Comment: Main + SM: 21 pages, 13 figures

Measuring fluctuations in matter's low energy excitations is the key to unveil the nature of the nonequilibrium response of materials. A promising outlook in this respect is offered by spectroscopic methods that address matter fluctuations by exploiting the statistical nature of light-matter interactions with weak few-photon probes. Here we report the first implementation of ultrafast phase randomized tomography, combining pump-probe experiments with quantum optical state tomography, to measure the ultrafast non-equilibrium dynamics in complex materials. Our approach utilizes a time-resolved multimode heterodyne detection scheme with phase-randomized coherent ultrashort laser pulses, overcoming the limitations of phase-stable configurations and enabling a robust reconstruction of the statistical distribution of phase-averaged optical observables. This methodology is validated by measuring the coherent phonon response in $\alpha$-quartz. By tracking the dynamics of the shot-noise limited photon number distribution of few-photon probes with ultrafast resolution, our results set an upper limit to the non-classical features of phononic state in $\alpha$-quartz and provide a pathway to access nonequilibrium quantum fluctuations in more complex quantum materials., Comment: 21 pages, 10 figures (including Supplementary Information)

Although entanglement is both a central ingredient in our understanding of quantum many-body systems and an essential resource for quantum technologies, we only have a limited ability to quantify entanglement in real quantum materials. Thus far, entanglement metrology in quantum materials has been limited to measurements involving Hermitian operators, such as the detection of spin entanglement using inelastic neutron scattering. Here, we devise a method to extract the quantum Fisher information (QFI) from non-Hermitian operators and formulate an entanglement witness for resonant inelastic x-ray scattering (RIXS). Our approach is then applied to the model iridate dimer system Ba$_3$CeIr$_2$O$_9$ and used to directly test for entanglement of the electronic orbitals between neighboring Ir sites. We find that entanglement is challenging to detect under standard conditions, but that it could be achieved by analyzing the outgoing x-ray polarization or via specific choices of momentum and energy. Our protocol provides a new handle for entanglement detection, which offers routes to related types of entanglement witness (such as orbitally-resolved measurements) and to the generalization to out-of-equilibrium settings accessed in ultrafast settings., Comment: 10 pages, 8 figures

The nature of the "failed" ferroelectric transition in SrTiO3 has been a long-standing puzzle in condensed matter physics. A compelling explanation is the competition between ferroelectricity and an instability with a mesoscopic modulation of the polarization. These polarization density waves, which should become especially strong near the quantum critical point, break local inversion symmetry and are difficult to probe with conventional x-ray scattering methods. Here we combine a femtosecond x-ray free electron laser (XFEL) with THz coherent control methods to probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization on nanometer lengthscales in SrTiO3. We find polar-acoustic collective modes that are soft particularly at the tens of nanometer lengthscale. These precursor collective excitations provide evidence for the conjectured mesoscopic modulated phase in SrTiO3.

We introduce phonon state tomography (PST) as a diagnostic probe of electron dynamics in solids whose phonons are optically excited by a laser pulse at initial time. Using a projected-purified matrix-product states algorithm, PST decomposes the exact correlated electron-phonon wavefunction into contributions from purely electronic states corresponding to statistically typical configurations of the optically accessible phononic response, enabling a 'tomographic' reconstruction of the electronic dynamics generated by the phonons. Thus, PST may be used to diagnose electronic behavior in experiments that access only the phonon response, such as thermal diffuse x-ray and electron scattering. We study the dynamics of a metal whose infrared phonons are excited by an optical pulse at initial time and use it to simulate the sample-averaged momentum-resolved phonon occupancy and accurately reconstruct the electronic correlations. We also use PST to analyze the influence of different pulse shapes on the light-induced enhancement and suppression of electronic correlations., Comment: Added one paragraph to the main text and uploaded the Supporting Information

Excitons are the neutral quasiparticles that form when Coulomb interactions create bound states between electrons and holes. Due to their bosonic nature, excitons are expected to condense and exhibit superfluidity at sufficiently low temperatures. In interacting Chern insulators, excitons may inherit the nontrivial topology and quantum geometry from the underlying electron wavefunctions. We theoretically investigate the excitonic bound states and superfluidity in flat-band insulators pumped with light. We find that the exciton wavefunctions exhibit vortex structures in momentum space, with the total vorticity being equal to the difference of Chern numbers between the conduction and valence bands. Moreover, both the exciton binding energy and the exciton superfluid density are proportional to the Brillouin-zone average of the quantum metric and the Coulomb potential energy per unit cell. Spontaneous emission of circularly polarized light from radiative decay is a detectable signature of the vorticity of excitons. We propose that the exciton vorticity can also be experimentally measured by the nonlinear anomalous Hall effect, whereas the exciton superfluidity can be detected by voltage-drop quantization through a combination of the quantum geometry and the Aharonov-Casher effect. Topological excitons and their superfluid phase could be realized in flat bands of twisted Van der Waals heterostructures., Comment: 25+3 pages, 3 figures

Doped SrTi1-xNbxO3 exhibits superconductivity and a mid-infrared optical response reminiscent of copper-oxide superconductors. Strangely, its plasma frequency, omega_p, increases by a factor of ~3 when cooling from 300 K to 20 K, without any accepted explanation. Here, we present momentum-resolved electron energy loss spectroscopy (M-EELS) measurements of SrTi1-xNbxO3 at nonzero momentum, q. We find that the infrared feature previously identified as a plasmon is present at large q in insulating SrTiO3, where it exhibits the same temperature dependence and may be identified as an anharmonic, multiphonon background. Doping with Nb increases its peak energy and total spectral weight, drawing this background to lower q where it becomes visible in IR optics experiments. We conclude that the "plasmon" in doped SrTi1-xNbxO3 is not a free-carrier mode, but a composite excitation that inherits its unusual properties from the lattice anharmonicity of the insulator., Comment: 5 pages, 4 figures

Characterizing and controlling entanglement in quantum materials is crucial for the development of next-generation quantum technologies. However, defining a quantifiable figure of merit for entanglement in macroscopic solids is theoretically and experimentally challenging. At equilibrium the presence of entanglement can be diagnosed by extracting entanglement witnesses from spectroscopic observables and a nonequilibrium extension of this method could lead to the discovery of novel dynamical phenomena. Here, we propose a systematic approach to quantify the time-dependent quantum Fisher information and entanglement depth of transient states of quantum materials with time-resolved resonant inelastic x-ray scattering. Using a quarter-filled extended Hubbard model as an example, we benchmark the efficiency of this approach and predict a light-enhanced many-body entanglement due to the proximity to a phase boundary. Our work sets the stage for experimentally witnessing and controlling entanglement in light-driven quantum materials via ultrafast spectroscopic measurements., Comment: 15 pages, 10 figures

Many-body entanglement in condensed matter systems can be diagnosed from equilibrium response functions through the use of entanglement witnesses and operator-specific quantum bounds. Here, we investigate the applicability of this approach for detecting entangled states in quantum systems driven out of equilibrium. We use a multipartite entanglement witness, the quantum Fisher information, to study the dynamics of a paradigmatic fermion chain undergoing a time-dependent change of the Coulomb interaction. Our results show that the quantum Fisher information is able to witness distinct signatures of multipartite entanglement both near and far from equilibrium that are robust against decoherence. We discuss implications of these findings for probing entanglement in light-driven quantum materials with time-resolved optical and x-ray scattering methods., Comment: 8 pages, 4 figures

While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-$T_c$ superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen $K$-edge, we studied the EPC in Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ (Bi2212) and Nd$_{1+x}$Ba$_{2-x}$Cu$_3$O$_{7-\delta}$ (NBCO) at different doping levels ranging from heavily underdoped ($p =0.07$) to overdoped ($p=0.21$). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO$_3$ chains and the CuO$_2$ planes. Combining the results from the two families, we find the EPC strength decreases with doping at $\mathbf{q_\parallel}=(-0.25, 0)$ r.l.u., but has a non-monotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave (CDW) excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in $d$-wave pairing., Comment: 10 pages, 5 figures

Understanding the nature of charge density waves (CDW) in cuprate superconductors has been complicated by material specific differences. A striking example is the opposite doping dependence of the CDW ordering wavevector in La-based and Y-based compounds, the two families where charge ordering is strongest and best characterized. Here we report a combined resonant soft X-ray scattering (RSXS) and neutron scattering study of charge and spin density waves in isotopically enriched La$_{1.8-x}$ Eu$_{0.2}$ Sr$_{x}$ CuO$_{4}$ over a range of doping $0.07 \leq x \leq 0.20$. For all dopings studied by RSXS, we find that the CDW amplitude is approximately temperature-independent and develops well above experimentally accessible temperatures. Surprisingly, the CDW ordering wavevector shows a non-monotonic temperature dependence, with a sudden change occurring at temperatures near the SDW onset temperature. We describe this behavior with a Landau-Ginzburg theory for an incommensurate CDW in a metallic system with a finite charge compressibility and CDW-SDW coupling. Our Landau-Ginzburg analysis suggests that the ordering wavevector at high temperatures decreases with increased doping. This behavior is opposite to the trend at low temperatures and highly reminiscent of the doping dependence seen in YBa$_2$ Cu$_3$ O$_{6+\delta}$ , suggesting a common origin of the CDW in hole-doped cuprate superconductors., Comment: Manuscript submitted to PNAS; ArXiv version formatted in Revtex4-2; Supplementary Material included as appendices; 20 pages, 14 figures (6 in the main text), and 41 references

Neutron diffraction on the centrosymmetric square-net magnet EuGa$_2$Al$_2$ reveals multiple incommensurate magnetic states (AFM1,2,3) in zero field. In applied field, a new magnetic phase (A) is identified from magnetization and transport measurements, bounded by two of the $\mu_0H$~=~0 incommensurate magnetic phases (AFM1,helical and AFM3, cycloidal) with different moment orientations. Moreover, magneto-transport measurements indicate the presence of a topological Hall effect, with maximum values centered in the A phase. Together, these results render EuGa$_2$Al$_2$ a material with non-coplanar or topological spin texture in applied field. X-ray diffraction reveals an out-of-plane (OOP) charge density wave (CDW) below $T_{CDW} \sim$ 50 K while the magnetic propagation vector lies in plane below $T_N$ = 19.5 K. Together these data point to a new route to realizing in-plane non-collinear spin textures through an OOP CDW. In turn, these non-collinear spin textures may be unstable against the formation of topological spin textures in an applied field.

Ultrafast lasers are an increasingly important tool to control and stabilize emergent phases in quantum materials. Among a variety of possible excitation protocols, a particularly intriguing route is the direct light-engineering of microscopic electronic parameters, such as the electron hopping and the local Coulomb repulsion (Hubbard $U$). In this work, we use time-resolved x-ray absorption spectroscopy to demonstrate the light-induced renormalization of the Hubbard $U$ in a cuprate superconductor, La$_{1.905}$Ba$_{0.095}$CuO$_4$. We show that intense femtosecond laser pulses induce a substantial redshift of the upper Hubbard band, while leaving the Zhang-Rice singlet energy unaffected. By comparing the experimental data to time-dependent spectra of single- and three-band Hubbard models, we assign this effect to a $\sim140$ meV reduction of the onsite Coulomb repulsion on the copper sites. Our demonstration of a dynamical Hubbard $U$ renormalization in a copper oxide paves the way to a novel strategy for the manipulation of superconductivity, magnetism, as well as to the realization of other long-range-ordered phases in light-driven quantum materials., Comment: 13 pages, 7 figures

We recently reported [1,2] measurements of the charge density fluctuations in the strange metal cuprate Bi$_{2.1}$Sr$_{1.9}$Ca$_{1.0}$Cu$_{2.0}$O$_{8+x}$ using both reflection M-EELS and transmission EELS with $\leq$10 meV energy resolution. We observed the well-known 1 eV plasmon in this material for momentum $q\lesssim$ 0.12 r.l.u., but found that it does not persist to large $q$. For $q\gtrsim0.12$ r.l.u., we observe a frequency-independent continuum, similar to that observed in early Raman scattering experiments [3,4], that correlates highly with the strange metal phase [2]. In his Comment (arXiv:2103.10268), Joerg Fink claims we do not see the plasmon, and that our results are inconsistent with optics, RIXS, and the author's own transmission EELS measurements with $\sim$100 meV resolution from the early 1990's [5,6]. The author claims we have made a trigonometry error and are measuring a larger momentum than we think. The author asserts that the two-particle excitations of cuprate strange metals are accurately described by weakly interacting band theory in RPA with corrections for conduction band carrier lifetimes and Umklapp effects. Here, we show that the author's Comment is in contradiction with known information from the literature. At $q\lesssim0.12$ r.l.u. we see the same 1 eV plasmon as other techniques. Moreover we compute our momentum correctly, adjusting the sample and detector angles during an energy scan to keep $q$ fixed. The only discrepancy is between our data and the results of Ref. [5] for $q\gtrsim0.12$ r.l.u. where, because of the coarse resolution used, the data had to be corrected for interference from the elastic line. A reexamination of these corrections in early transmission EELS measurements would likely shed light on this discrepancy., Comment: 5 pages, 3 figures. Response to arXiv:2103.10268. Wording updated in selected locations

Identifying what broken symmetries are present in the cuprates has become a major area of research. Many authors have reported evidence for so-called "$Q \sim 0$" order that involves broken inversion, mirror, chiral, or time-reversal symmetry that is uniform in space. Not all these observations are well understood and new experimental probes are needed. Here we use resonant soft x-ray scattering (RSXS) to search for $Q \sim 0$ order in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ (Bi-2212) by measuring the region of a forbidden Bragg peak, $(0,0,3)$, which is normally extinguished by symmetry but may become allowed on resonance if valence band order is present. Using circularly polarized light, we found that this reflection becomes allowed on the Cu $L_3$ resonance for temperatures $T_c < T < T^\ast$, though remains absent in linear polarization and at other temperatures. This observation suggests the existence of spatially uniform valence band order near the pseudogap temperature. In addition, we observed periodic oscillations in the specular reflectivity from the sample surface that resemble thin film interference fringes, though no known film is present. These fringes are highly resonant, appear in all polarizations, and exhibit a period that depends on the location where the beam strikes the sample surface. We speculate that these fringes arise from interaction between some intrinsic valence band instability and extrinsic structural surface morphologies of the material. Our study supports the existence of some kind of $Q \sim 0$ broken symmetry state in Bi-2212 at intermediate temperatures, and calls for further study using a microfocused beam that could disentangle microscopic effects from macroscopic heterogeneities., Comment: 9 pages, 4 figures

Manipulating spin fluctuations with ultrafast laser pulses is a promising route to dynamically control collective phenomena in strongly correlated materials. However, understanding how photoexcited spin degrees of freedom evolve at a microscopic level requires a momentum- and energy-resolved characterization of their nonequilibrium dynamics. Here, we study the photoinduced dynamics of finite-momentum spin excitations in two-dimensional Mott insulators on a square lattice. By calculating the time-resolved resonant inelastic x-ray scattering cross-section, we show that an ultrafast pump above the Mott gap induces a prompt softening of the spin excitation energy, compatible with a transient renormalization of the exchange interaction. While spin fluctuations in a hole-doped system (paramagnons) are well described by Floquet theory, magnons at half filling are found to deviate from this picture. Furthermore, we show that the paramagnon softening is accompanied by an ultrafast suppression of $d$-wave pairing correlations, indicating a link between the transient spin excitation dynamics and superconducting pairing far from equilibrium., Comment: 7 pages, 4 figures

How superconductivity interacts with charge or nematic order is one of the great unresolved issues at the center of research in quantum materials. Ba$_{1-x}$Sr$_{x}$Ni$_{2}$As$_{2}$ (BSNA) is a charge ordered pnictide superconductor recently shown to exhibit a six-fold enhancement of superconductivity due to nematic fluctuations near a quantum phase transition (at $x_c=0.7$). The superconductivity is, however, anomalous, with the resistive transition for $0.4 < x< x_c$ occurring at a higher temperature than the specific heat anomaly. Using x-ray scattering, we discovered a new charge density wave (CDW) in BSNA in this composition range. The CDW is commensurate with a period of two lattice parameters, and is distinct from the two CDWs previously reported in this material. We argue that the anomalous transport behavior arises from heterogeneous superconductivity nucleating at antiphase domain walls in this CDW. We also present new data on the incommensurate CDW, previously identified as being unidirectional, showing that is a rotationally symmetric, "4$Q$" state with $C_4$ symmetry. Our study establishes BSNA as a rare material containing three distinct CDWs, and an exciting testbed for studying coupling between CDW, nematic, and SC orders., Comment: 5 pages, 5 figures + supplemental material document

We employ Momentum-Resolved Electron Energy Loss Spectroscopy (M-EELS) on Bi2.1Sr1.9CaCu2O8+x to resolve the issue of the kink feature in the electron dispersion widely observed in the cuprates. To this end, we utilize the GW approximation to relate the density response function measured in in M-EELS to the self-energy, isolating contributions from phonons, electrons, and the momentum dependence of the effective interaction to the decay rates. The phononic contributions, present in the M-EELS spectra due to electron-phonon coupling, lead to kink features in the corresponding single-particle spectra at energies between 40 meV and 80 meV, independent of the doping level. We find that a repulsive interaction constant in momentum space is able to yield the kink attributed to phonons in ARPES. Hence, our analysis of the M-EELS spectra points to local repulsive interactions as a factor that enhances the spectroscopic signatures of electron-phonon coupling in cuprates. We conclude that the strength of the kink feature in cuprates is determined by the combined action of electron-phonon coupling and electron-electron interactions.

Ultrafast optical pulses are an increasingly important tool for controlling quantum materials and triggering novel photo-induced phase transitions. Understanding these dynamic phenomena requires a probe sensitive to spin, charge, and orbital degrees of freedom. Time-resolved resonant inelastic X-ray scattering (trRIXS) is an emerging spectroscopic method, which responds to this need by providing unprecedented access to the finite-momentum fluctuation spectrum of photoexcited solids. In this Perspective, we briefly review state-of-the-art trRIXS experiments on condensed matter systems, as well as recent theoretical advances. We then describe future research opportunities in the context of light control of quantum matter., Comment: 12 pages, 6 figures, Invited Perspective to appear in npg Communications Physics

We use femtosecond resonant soft x-ray scattering to measure the ultrafast optical melting of charge-order correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$. By analyzing both the energy-resolved and energy-integrated order parameter dynamics, we find evidence of a short-lived nonequilibrium state, whose features are compatible with a sliding charge density wave coherently set in motion by the pump. This transient state exhibits shifts in both the quasielastic line energy and its wave vector, as expected from a classical Doppler effect. The wave vector change is indeed found to directly follow the pump propagation direction. These results demonstrate the existence of sliding charge order behavior in an unconventional charge density wave system and underscore the power of ultrafast optical excitation as a tool to coherently manipulate electronic condensates., Comment: 8 pages, 9 figures, 39 references

Charge order is universal among high-T$_c$ cuprates but its relevance to superconductivity is not established. It is widely believed that, while static order competes with superconductivity, dynamic order may be favorable and even contribute to Cooper pairing. We use time-resolved resonant soft x-ray scattering to study the collective dynamics of the charge order in the prototypical cuprate, La$_{2-x}$Ba$_x$CuO$_4$. We find that, at energy scales $0.4$ meV $ \lesssim \omega \lesssim 2$ meV, the excitations are overdamped and propagate via Brownian-like diffusion. At energy scales below 0.4 meV the charge order exhibits dynamic critical scaling, displaying universal behavior arising from propagation of topological defects. Our study implies that charge order is dynamic, so may participate tangibly in superconductivity., Comment: 31 pages, 4 figures, 8 supplementary figures, revised paragraph formatting

We address the question of the mismatch between the zero momentum limits of the transverse and longitudinal dielectric functions for a fixed direction of the driving field observed in the cuprates. This question translates to whether or not the order in which the longitudinal and transverse momentum transfers are taken to zero commute. While the two limits commute for both isotropic and anisotropic Drude metals, we argue that a scaleless vertex interaction that depends solely on the angle between scattered electron momenta is sufficient to achieve non-commutativity of the two limits even for a system that is inherently isotropic. We demonstrate this claim for a simple case of the Drude conductivity modified by electron-boson interactions through appropriate vertex corrections, and outline possible consequences of our result to optical and electron energy loss spectroscopy (EELS) measurements close to zero momentum transfer, Comment: 7 pages, 1 figure including Supplemental Material

Ba(Ni$_{1-x}$Co$_x$)$_2$As$_2$ is a structural homologue of the pnictide high temperature superconductor, Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$, in which the Fe atoms are replaced by Ni. Superconductivity is highly suppressed in this system, reaching a maximum $T_c$ = 2.3 K, compared to 24 K in its iron-based cousin, and the origin of this $T_c$ suppression is not known. Using x-ray scattering, we show that Ba(Ni$_{1-x}$Co$_x$)$_2$As$_2$ exhibits a unidirectional charge density wave (CDW) at its triclinic phase transition. The CDW is incommensurate, exhibits a sizable lattice distortion, and is accompanied by the appearance of $\alpha$ Fermi surface pockets in photoemission [B. Zhou et al., Phys. Rev. B 83, 035110 (2011)], suggesting it forms by an unconventional mechanism. Co doping suppresses the CDW, paralleling the behavior of antiferromagnetism in iron-based superconductors. Our study demonstrates that pnictide superconductors can exhibit competing CDW order, which may be the origin of $T_c$ suppression in this system.

One of the most fundamental properties of an interacting electron system is its frequency- and wave-vector-dependent density response function, $\chi({\bf q},\omega)$. The imaginary part, $\chi''({\bf q},\omega)$, defines the fundamental bosonic charge excitations of the system, exhibiting peaks wherever collective modes are present. $\chi$ quantifies the electronic compressibility of a material, its response to external fields, its ability to screen charge, and its tendency to form charge density waves. Unfortunately, there has never been a fully momentum-resolved means to measure $\chi({\bf q},\omega)$ at the meV energy scale relevant to modern elecronic materials. Here, we demonstrate a way to measure $\chi$ with quantitative momentum resolution by applying alignment techniques from x-ray and neutron scattering to surface high-resolution electron energy-loss spectroscopy (HR-EELS). This approach, which we refer to here as "M-EELS," allows direct measurement of $\chi''({\bf q},\omega)$ with meV resolution while controlling the momentum with an accuracy better than a percent of a typical Brillouin zone. We apply this technique to finite-q excitations in the optimally-doped high temperature superconductor, Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi2212), which exhibits several phonons potentially relevant to dispersion anomalies observed in ARPES and STM experiments. Our study defines a path to studying the long-sought collective charge modes in quantum materials at the meV scale and with full momentum control., Comment: 26 pages, 10 sections, 7 figures, and an appendix

We modulate the atomic structure of bilayer graphene by driving its lattice at resonance with the in-plane E1u lattice vibration at 6.3um. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES) with extreme ultra-violet (XUV) pulses, we measure the response of the Dirac electrons near the K-point. We observe that lattice modulation causes anomalous carrier dynamics, with the Dirac electrons reaching lower peak temperatures and relaxing at faster rate compared to when the excitation is applied away from the phonon resonance or in monolayer samples. Frozen phonon calculations predict dramatic band structure changes when the E1u vibration is driven, which we use to explain the anomalous dynamics observed in the experiment., Comment: 16 pages, 8 figures

The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime., Comment: 18 pages, 6 figures

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a semiconducting bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy and momentum dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme ultra-violet (EUV) pulses at 31.5 eV photon energy to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. While excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find indication for carrier multiplication, questioning the applicability of graphene for light harvesting. Time-resolved photoemission spectroscopy in the EUV emerges as the technique of choice to assess the suitability of new materials for optoelectronics, providing quantitatively accurate measurements of non-equilibrium carriers at all energies and wavevectors., Comment: 16 pages, 7 figures

We present structural studies of V$_{1-x}$Cr$_x$O$_2$ (pure, 0.7% and 2.5% Cr doped) compounds at room temperature in a diamond anvil cell for pressures up to 20 GPa using synchrotron x-ray powder diffraction. All the samples studied show a persistence of the monoclinic $M_1$ symmetry between 4 and 12 GPa. Above 12 GPa, the monoclinic $M_1$ symmetry changes to isostructural $M_x$ phase (space group $P2_1/c$) with a significant anisotropy in lattice compression of the $b$-$c$ plane of the $M_{1}$ phase. This behavior can be reconciled invoking the pressure induced charge-delocalization.